CN110190200B - Efficient pure white light organic electroluminescent device with high color rendering index and preparation method thereof - Google Patents
Efficient pure white light organic electroluminescent device with high color rendering index and preparation method thereof Download PDFInfo
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- H10K50/131—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light comprising stacked EL layers within one EL unit with spacer layers between the electroluminescent layers
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Abstract
A pure white light organic electroluminescent device with high efficiency and high color rendering index and a preparation method thereof belong to the technical field of organic semiconductor luminescent devices. The device comprises a transparent substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode from bottom to top in sequence, wherein the light emitting layer is of a three-layer structure and comprises a red phosphorescent layer, a spacing layer and a non-doped blue fluorescent layer from bottom to top in sequence; the red phosphorescence layer is formed by doping a red phosphorescence object material with a green thermal activation delayed fluorescence host material. The invention selects the aggregation-induced emission material with excellent performance as the blue light layer, the high-efficiency thermal activation delayed fluorescence material as the host of the green light layer and the red phosphorescence material, and prepares the pure white light organic electroluminescent device with simple device structure, simple manufacturing process, low cost, high efficiency and high color rendering index by utilizing incomplete energy transfer between the host and the object, thereby being beneficial to the commercial application.
Description
Technical Field
The invention belongs to the technical field of organic semiconductor light-emitting devices, and particularly relates to a pure white light organic electroluminescent device with high efficiency and high color rendering index and a preparation method thereof.
Background
The organic light emitting diode (O L ED) is considered to be a next generation novel display and illumination technology capable of replacing inorganic light emitting diodes due to the advantages of flexibility, wide viewing angle, energy conservation, high response speed and the like, and the white organic light emitting diode (WO L ED) can complement a short board of the inorganic O L ED illumination technology and is a main force of the next generation illumination technology.
According to the different types of luminescent materials in the luminescent layer, O L ED can be divided into total fluorescence, total phosphorescence and fluorescence/phosphorescence sensitization WO L ED. to total fluorescence WO L ED, although the total fluorescence and phosphorescence have long service life, the efficiency is generally low, the total phosphorescence WO L ED is limited to the scarcity of heavy metal resources, and the stability of blue phosphorescence material is poor, which is not good for commercial development.
The Color Rendering Index (CRI) is an important parameter for measuring the quality of a light source, and refers to the fidelity of the light source to the Color of an object. The CRI is in the range of 0-100, and the CRI of an ideal light source is 100, which is the same as that of sunlight or an incandescent lamp. For commercial lighting, CRI's in excess of 80 are generally required, and higher CRI (>90) are required in museums, exhibitions or in gorgeous studio halls.
Unlike monochromatic O L ED, WO L ED has a broad spectrum, and WO L ED with a high CRI covers as much as possible of the visible light band of 400-780nm, according to the theory of colorimetry, the (0.3333 ) in the CIE (International Commission on illumination) coordinates is called the color coordinates of energy points such as white light, etc. WO L ED reported at present is basically warm white light or yellow white light, and has poor color reduction capability.
Therefore, the development of a pure white light WO L ED with simple process, low cost, and high efficiency and CRI is of great significance to promote the commercialization of the white light O L ED.
Disclosure of Invention
In order to solve the above problems, an object of the present invention is to provide a pure white organic electroluminescent device and a method for manufacturing the same, wherein a collection-induced luminescent material with excellent performance is selected as a blue layer, a thermally activated delayed fluorescent material with high efficiency is selected as a host of a green layer and a red phosphorescent material, incomplete energy transfer between the host and the guest is utilized to prepare the pure white organic electroluminescent device with a simple device structure, a simple manufacturing process, low cost, high efficiency and a high color rendering index, thereby facilitating commercial application.
The invention relates to a high-efficiency high-color rendering index pure white light organic electroluminescent device which sequentially comprises a transparent substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode from bottom to top, wherein the light emitting layer is of a three-layer structure and sequentially comprises a red phosphorescence layer, a spacing layer and a non-doped blue fluorescent layer from bottom to top; the red phosphorescence layer is formed by doping a red phosphorescence object material with a green thermal activation delayed fluorescence host material.
Furthermore, the thickness of the red phosphorescent material layer is 0.1-30 nm, the thickness of the spacing layer is 1-10 nm, the thickness of the undoped blue fluorescent material layer is 0.1-40 nm, and the thickness range of the rest layers is less than or equal to 40 nm.
Further, the pure white organic electroluminescent device can show each component to emit light by incomplete energy transfer between a host and an object under the condition of very low doping concentration. The undoped blue fluorescent material generates blue light, the green thermal activation delayed fluorescent material host generates green light, the sensitized red phosphorescent guest material generates red light, and multi-color spectrum complementation is performed to obtain red-green-blue three-color pure white light emission with high CRI.
Furthermore, the undoped blue fluorescent material is N, N-diphenyl-4- (10- (4- (1, 2-triphenylethylene) phenyl) anthracene-9-yl) aniline (TPAATPE, CN109608403A), is an excellent aggregation-induced luminescent material, and has high luminous efficiency and good stability.
Further, the spacer layer can be divided into a hole type spacer layer, an electron type spacer layer or a mixture of two bipolar spacer layers. The triplet state energy level of the spacer material is larger than that of the green thermal activation delayed fluorescence host material and the red phosphorescence guest material, so that the energy transfer between the fluorescence material and the phosphorescence material can be better prevented, and the triplet state excitons and singlet state excitons generated by the device are effectively utilized, thereby ensuring the high efficiency of the device.
Further, the spacer layer material is a cavity type 4,4' -cyclohexyl di [ N, N-di (4-methylphenyl) aniline](TAPC), or a cavitated 4,4' -cyclohexylbis [ N, N-bis (4-methylphenyl) aniline](TAPC) and electronic bis (2- (2-hydroxyphenyl) -pyridine) beryllium (Bepp)2) The mass ratio is 1: 1, a hybrid bipolar spacer layer.
Further, the green thermal activation delayed fluorescence host material is 10- (4-, (Diphenylboron) phenyl) -10H-Phenothiazines (PTZMES)2B, front. chem.2019,7,373, compared to conventional fluorescent materials, the thermally activated delayed fluorescent material has a small difference in singlet and triplet energy levels, and cross-over between the triplet excitons and the singlet inversion system can occur at room temperature, and internal quantum efficiency close to 100% is achieved by using the triplet excitons. In addition, the material has excellent carrier transport capability, and can be used as a main body of bipolar transport to sensitize a phosphorescent material; and the triplet state energy level is larger than that of the red phosphorescent guest material, so that the energy return from the guest to the host can be prevented.
Further, the red phosphorescent guest material is (1-phenylisoquinoline-C2, N) iridium (III) (Ir (piq))3) The luminescent layer is prepared by a host-guest doping technology, and the luminescent layer is host PTZMES by utilizing an incomplete host-guest energy transfer mechanism2B producing a green, red phosphorescent guest material Ir (piq)3Producing a corresponding red light. The device performance is adjusted by adopting the multicolor organic luminescent material, the complementation of multicolor spectrum is carried out, the CRI of the device is obviously improved, and the commercialization of the device is facilitated.
Furthermore, the doping concentration of the red phosphorescent guest material is 0.01-10%, and preferably 0.1-5%.
Further, the substrate is transparent conductive glass, the anode is Indium Tin Oxide (ITO), the hole injection layer is 2, 3, 6, 7,10, 11-hexacyano-1, 4, 5, 8, 9, 12-Hexaazatriphenylene (HATCN), the hole transport layer is TAPC, and the exciton blocking layer is tris (4-carbazole-9-phenyl) amine (TCTA).
Furthermore, the cathode is an Al film, the electron injection layer is lithium fluoride (L iF), and the electron transport layer is 3, 3', 5,5 ' -4 (3-pyridyl) -1,1':3', 1' -terphenyl (BmPyPB).
Compared with the prior art, the invention has the beneficial effects that:
the pure white light organic electroluminescent device with high efficiency and high color rendering index selects the aggregation-induced luminescent material with excellent performance as the blue layer, the high-efficiency thermal activation delayed fluorescent material as the green layer and the host to sensitize the red phosphorescent material, utilizes an incomplete energy transfer mechanism between the host and the guest, adopts the multicolor organic luminescent material to adjust the light color of the device, performs the complementation of multicolor spectrum, obviously improves the CRI of the device, and is beneficial to the commercial application.
In addition, the structure and the material of the white light organic electroluminescent device are optimized, and the pure white light organic electroluminescent device with simple device structure and manufacturing process, low cost, high efficiency and high color rendering index is prepared.
The raw materials mentioned in the invention are all commercially available or prepared according to known literature or patents, and the molecular structural formula is shown as follows:
drawings
Fig. 1 is a schematic structural view of a pure white organic electroluminescent device of example 1;
FIG. 2 is a schematic structural view of a pure white organic electroluminescent device of example 2;
FIG. 3 is a schematic structural view of a pure white organic electroluminescent device of example 3;
FIG. 4 is a current density-voltage-luminance characteristic curve of a pure white organic electroluminescent device of example 1;
fig. 5 is a current efficiency-luminance-energy efficiency characteristic curve of a pure white organic electroluminescent device of example 1;
FIG. 6 is an external quantum efficiency-luminance characteristic curve and normalized electroluminescence spectra, CIE and CRI of the pure white organic electroluminescent device of example 1;
FIG. 7 is an external quantum efficiency-luminance characteristic curve and normalized electroluminescence spectra, CIE and CRI of the warm white organic electroluminescent device of example 2;
fig. 8 is an external quantum efficiency-luminance characteristic curve and normalized electroluminescence spectra, CIE and CRI of the pure white organic electroluminescent device of example 3.
Detailed Description
The present invention is further described below in conjunction with the appended drawings to facilitate an understanding of the present invention by those skilled in the art. It is obvious that the embodiments described are only a part of the experiments and not all embodiments, and those skilled in the art should be able to make non-essential modifications, equivalent replacements and improvements of the present invention according to the above-mentioned disclosure within the protection scope of the present invention. The starting materials mentioned below are either commercially available or prepared according to known literature or patents, and the process steps and preparation methods not mentioned are those well known to the person skilled in the art.
Example 1
A white light organic electroluminescent device W1, the structure of the device W1 is: ITO/HAT-CN (5nm)/TAPC (35nm)/TCTA (5nm)/PTZMES2B：Ir(piq)3(12nm，0.5％)/TAPC(4 nm)/TPAAnTPE(8nm)/BmPyPB(40nm)/LiF(1nm)/Al。
First, a cavity type spacer layer is selected, the spacer layer is made of TAPC, and as shown in fig. 1, the structure of the device W1 is stacked by the following functional layers from bottom to top: the organic electroluminescent device comprises a substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a red phosphorescent material layer, a hole type spacing layer, a blue fluorescent material layer, an electron transport layer, an electron injection layer and a cathode. The preparation method comprises the following steps:
1. preparing an ITO thin plate as an anode on the substrate conductive glass in a sputtering mode;
2. and sequentially cleaning the ITO conductive glass with deionized water, isopropanol, acetone, toluene, acetone and isopropanol in an ultrasonic bath for 20 minutes respectively, and drying in an oven for later use. Treating the surface of the ITO glass in an ultraviolet ozone cleaning machine for 40 minutes, and then transferring the ITO glass into vacuum evaporation equipment;
3. vacuum evaporating a hole injection layer HATCN on the anode ITO conductive glass, wherein the thickness of the hole injection layer HATCN is 5 nm;
4. vacuum evaporating a hole transport layer TAPC (tantalum polycarbonate) on the HATCN, wherein the thickness of the hole transport layer TAPC is 35 nm;
5. evaporating an exciton blocking layer TCTA on TAPC, wherein the thickness is 5 nm;
6. on top of TCTA, a light emitting layer is evaporated: the luminescent layer is a red phosphor layer PTZMES2B：Ir(piq)3(12nm，PTZMes2B is a host fluorescent material, Ir (piq)3The material is an object phosphorescent material, and the doping concentration of the object material in the total mass is 0.5 percent), the cavity type spacing layer TAPC (4nm) and the undoped blue light fluorescent layer TPAATPE (8 nm);
7. an electron transport layer BmPyPB is evaporated on the luminescent layer, and the thickness is 40 nm;
8. an electron injection layer L iF is evaporated on the BmPyPB with the thickness of 1 nm;
9. on top of L iF, cathode Al was evaporated to a thickness of 100 nm.
For the device W1 prepared as described above, the delayed fluorescence material PTZMES was activated in green color by heat2B is doped with red phosphorescent material Ir (piq)3Each of the components is capable of exhibiting its own luminescence, PTZMes, at very low doping concentrations, using incomplete energy transfer between host and guest2B produces green light, Ir (piq)3Corresponding red light is generated, the complementation of multicolor spectrum is carried out, and the red-green-blue three-color pure white light emission with high CRI can be obtained. As shown in fig. 4 to 6, under the condition that the efficiency of the device is still high (the external quantum efficiency is 25.3%), the electroluminescence spectrum of the device almost covers the whole visible light region, and the ultrahigh CRI (92) is obtained, and the CIE coordinates are (0.34, 0.38), and the color coordinates (0.3333 ) close to the energy points of white light and the like can be classified as the emission of pure white light. The high-efficiency white light device reported at present is almost warm white light, and has weak color reduction capability, and the pure white light electroluminescent device with high efficiency and high CRI reported by the invention fills the blank of the field.
Example 2
The device structure and the preparation material of the white light device W1 are kept unchanged, and the hole type spacing layer TAPC in the luminescent layer is changed into the electron type spacing layer Bepp2And the thickness is 4 nm. A white light device W2 was prepared, the structure of which was: ITO/HATCN (5nm)/TAPC (35nm)/TCTA (5nm)/PTZMES2B：Ir(piq)3(12nm， 0.5％)/Bepp2(4nm)/TPAATPE(8nm)/BmPyPB(40nm)/LiF(1nm)/Al。
As shown in fig. 2, the structure of the device W2 is moved from bottom to top in the order of the following functional layers superimposed: a substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a red phosphorescent material layer, an electron type spacer layer, a blue fluorescent material layer, an electron transport layer, an electron injection layer and a cathode. The preparation method is similar to example 1.
As shown in fig. 7, since an electron type spacer layer is used, electrons more easily pass through the spacer layer to reach the red phosphor layer, and the recombination region of excitons moves from the blue layer to the red layer, so that the blue component is reduced, the CRI is slightly lowered, but the external quantum efficiency of the device still reaches 20%. Moreover, the maximum luminance of the device exceeds 20000 cd m-2。
Example 3
The structure and preparation material of the white light device W1 are kept unchanged, and the hole type spacing layer TAPC in the luminescent layer is changed into a hole type material TAPC and an electron type material Bepp2A mixed bipolar spacer layer. TAPC and Bepp2The mass ratio of the two is 1: 1, with a thickness of 4nm, a white light device W3 was prepared, which had the structure: ITO/HATCN (5nm)/TAPC (35nm)/TCTA (5nm)/PTZMES2B： Ir(piq)3(12nm，0.5％)/TAPC：Bepp2(4nm，1：1)/TPAATPE(8nm)/BmPyPB(40 nm)/LiF(1nm)/Al。
As shown in fig. 3, the structure of the device W3 is moved from bottom to top in the order of the following functional layers superimposed: the organic electroluminescent device comprises a substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a red phosphorescent material layer, a bipolar spacing layer, a blue fluorescent material layer, an electron transport layer, an electron injection layer and a cathode. The preparation method is similar to example 1.
As shown in fig. 8, when the bipolar spacer layer is used, the device has the effect similar to that of the hole-type spacer layer, the maximum external quantum efficiency is 20.8%, the CRI is 92, and the maximum brightness of the device is also improved in the pure white range.
Example 2 the resulting device had little blue light content and was already in the warm white range, and thus the device did not belong to a pure white device. Then a suitable spacer layer for the device of the present invention would be a hole type spacer layer or a bipolar spacer layer.
Detailed electroluminescent performance data for the devices of all examples of the invention are listed in table 1.
Table 1: electroluminescent property data of the devices W1, W2, W3
The above-described embodiments are preferred embodiments of the present invention, and non-essential modifications, equivalents, improvements and the like, which are made by those skilled in the art without departing from the technical principles of the present invention, are intended to be included within the scope of the present invention.
Claims (5)
1. A high-efficiency pure white light organic electroluminescent device with high color rendering index is characterized in that: the organic electroluminescent device comprises a transparent substrate, an anode, a hole injection layer, a hole transport layer, an exciton blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode in sequence from bottom to top, wherein the light emitting layer is of a three-layer structure and comprises a red phosphorescent material layer, a spacing layer and a non-doped blue fluorescent material layer in sequence from bottom to top; the red phosphorescent material layer is made of a red phosphorescent guest material sensitized by doping of a green thermal activation delayed fluorescence host material; wherein the non-doped blue fluorescent material is N, N-diphenyl-4- (10- (4- (1, 2-triphenylethylene) phenyl) anthracene-9-yl) aniline; the spacer material is a hole-type 4,4' -cyclohexyl-bis [ N, N-bis (4-methylphenyl) aniline]Or 4,4' -cyclohexylbis [ N, N-bis (4-methylphenyl) aniline of the cavityle type]And electronic type bis (2- (2-hydroxyphenyl) -pyridine) beryllium in a mass ratio of 1: 1, a hybrid bipolar spacer layer; the green thermal activation delayed fluorescence host material is 10- (4- (diphenyl boron) phenyl) -10H-phenothiazine; the sensitized red phosphorescent guest material is trihydroxymethyl aminomethane (1-phenylisoquinoline-C)2And N) iridium (III), wherein the doping amount of the sensitized red phosphorescent guest material is 0.01-10% of the mass sum of the green thermally activated delayed fluorescence host material and the sensitized red phosphorescent guest material.
2. A pure white organic electroluminescent device with high efficiency and high color rendering index as claimed in claim 1, wherein: the thickness of the non-doped blue fluorescent material layer is 0.1-40 nm.
3. A pure white organic electroluminescent device with high efficiency and high color rendering index as claimed in claim 1, wherein: the thickness of the spacer layer is 1 to 10 nm.
4. A pure white organic electroluminescent device with high efficiency and high color rendering index as claimed in claim 1, wherein: the doping amount of the sensitized red phosphorescent guest material is 0.1-5% of the mass sum of the green thermally activated delayed fluorescence host material and the sensitized red phosphorescent guest material.
5. A pure white organic electroluminescent device with high efficiency and high color rendering index as claimed in claim 1, wherein: the thickness of the red phosphor layer is 0.1-30 nm.
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| CN111916569B (en) * | 2020-06-23 | 2022-01-18 | 华南理工大学 | Full-fluorescence white-light organic light emitting diode and preparation method thereof |
| CN111785851B (en) | 2020-07-16 | 2023-12-26 | 京东方科技集团股份有限公司 | WOLED device, manufacturing method thereof and WOLED display device |
| CN113036047B (en) * | 2021-03-08 | 2022-04-22 | 上海大学 | OLED plant growth light source and preparation method thereof |
| CN113066935A (en) * | 2021-03-16 | 2021-07-02 | 吉林大学 | White organic electroluminescent device with double-excited-base compound as main body |
| CN113451523B (en) * | 2021-07-05 | 2023-04-18 | 太原理工大学 | White light organic light emitting diode with full fluorescence emission |
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